Absorbing aerosols exert a warming or a cooling effect on the Earth’s system, depending on the circumstances. The direct radiative effect (DRE) of absorbing aerosols is negative (cooling) at the top-of-the-atmosphere (TOA) over a dark surface like the ocean, as the aerosols increase the planetary albedo, but it is positive (warming) over bright backgrounds like clouds. Furthermore, radiation absorption by aerosols heat the atmosphere locally, and, through rapid adjustments of the atmospheric column and cloud dynamics, the net effect can be amplified considerably. We developed a technique to study the absorption of radiation of smoke over low lying clouds using satellite spectrometry. The TOA DRE of smoke over clouds is large and positive over the southeast Atlantic Ocean off the west coast of Africa, which can be explained by the large decrease of reflected radiation by a polluted cloud, especially in the UV. However, general circulation models (GCMs) fail to reproduce these strong positive DRE, and in general GCMs disagree on the magnitude and even sign of the aerosol DRE in the southeast Atlantic region. Our satellite-derived DRE measurements show clear seasonal and inter-annual variations, consistent with other satellite measurements, which are not reproduced by GCMs. A comparison with model results showed discrepancies with the Ångström exponent of the smoke aerosols, which is larger than assumed in simulations, and a sensitivity to emission scenarios. However, this was not enough to explain the discrepancies, and we suspect that the modeling of cloud distributions and microphysics will have the necessary larger impact on DRE that will explain the differences between observations and modeling.